- Photonics Research
- Vol. 9, Issue 4, 484 (2021)
Abstract
1. INTRODUCTION
Chirality is of great importance in fundamental science, material design, biomedicine, and so on. Chiral optics associated with natural chiral molecules is limited by the fixed geometrical structure and weak optical signal mainly in the ultraviolet (UV) range. Plasmonic clusters supporting localized surface plasmon resonances (LSPRs) interact with visible light strongly, which can be controlled by the shape, size, position, and permittivity of the objects [1]. Plasmonic nanostructures can be precisely designed with complex geometric patterns and thus provide many opportunities for exploring light–matter/structure interaction, in particular the chiral nature of photonics. In the past decade, many types of chiral clusters have been explored to study circular dichroism (CD), such as helical particles [2,3], tetramers [4], hybrid L-shaped resonators [5], U-shaped antennas [6,7], hybrid rod-sphere structures [8], various dimers [9–14], and others [15,16]. Using intrinsic chiral clusters as building blocks, chiral metamaterials/metasurfaces [17–23] can discriminate right- and left-circularly polarized (RCP and LCP) light, and they can even realize selective transmission of different circularly polarized light [24–26]. Furthermore, 2D planar metasurfaces with extrinsic chirality can realize asymmetric transmission/reflection [27–30] as well as modulation of light’s wavefront, direction, and polarization [31–34], which is promising in developing metalenses. The responses of metasurfaces of stacked layers are discussed in the view of photonic systems [19,20,35,36]. Besides designing nanostructures, a structured light field (superchiral light) [37,38] is proposed to increase light–material interaction, which is promising in amplification of chiral molecules’ CD signal [39].
Collective effects {such as lattice resonance (LR) [40–44]} and interference effects (such as Fano resonance [45] and electromagnetic induced transparency) modulated by electromagnetic (EM) field phase play important roles in controlling the optical properties. However, the study of the combination of those effects in the chiral metasurface area is in the preliminary stage [22,46–51]. Many important issues need systematic studies. For example, it is known that the geometric configuration, such as the relative orientation/position of the substructure, affects the collective resonance [43,50,52], phases of the EM field {Pancharatnam–Berry (PB) [31,53,54] and propagation phase}, and mirror symmetry breaking (related to chiral response) [4,14,52]. Much effort is needed to investigate the physical consequence of the interplay of these effects, the resulting (chiral) optical properties, the applications in optics modulation, and device design.
Here we take an archetypical chiroptical nanorod dimer [9,55] as the building block of the metasurfaces to explore the combination effects of collective resonance and interference on the chiral optics. Using an analytical approach based on a coupled dipole model (CDM) and finite-difference time-domain (FDTD) simulation, we find that the optical chirality of the metasurface is dramatically increased by the coupling between LSPRs and LR. The collective effect results in significant chiral signal, even for metasurfaces made of achiral unit cell-orthogonal nanorod dimers. By using phase (PB phase and propagation phase) modulated LR, different chiral responses can be obtained; in particular, chirality-selective transparency [100% transmission and a g-factor of absorption up to 1.99 (close to the upper limit of 2)] associated with Wood’s anomaly is realized in a specially designed structure, though in general the interlayer coupling destroys the Wood’s anomaly. Our studies reveal a new mechanism of tuning the chiral optical properties based on collective effect assisted by phase modulation (PB phase and propagation phase), and the analytical results (verified by numerical simulation) clearly reveal the quantitative relationship between the geometry configuration and chiral optical responses, providing modern photonic applications such as circular polarizers, optical communication, and quantum information processing.
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The paper is organized as follows. First we introduce the analytical formula to calculate the transmittance of metasurfaces. Second, we discuss the chirality of twisted nanorods and LR in monolayer metasurfaces. Third, bilayer metasurfaces’ extraordinary chiral transmission induced by LR is discussed and the general relationship between geometry and chiral optical response is given. Finally, we discuss the extraordinary chiral transmission of cases with higher-order resonance, square lattices, and the optical activity beyond the coupled dipole limit.
2. THEORETICAL FORMULA
A. Coupled Dipole Model
Figure 1.Scheme of the metasurface made of arrays of twisted nanorod dimers.
For simplicity, the silver nanorods are modeled as ellipsoids, whose long- and short-axis radii are 80 and 30 nm. The longitudinal and transverse LSPRs’ resonance wavelengths are at 590 and 355 nm. In the wavelength range 450–700 nm, the dominant mode is due to longitudinal LSPR. Thus, the component of the dipole polarizability tensor along the long axis of the nanorod is considered. Higher-order multipole modes and transverse dipole modes are neglected. Furthermore, the distance between two rods in the nearby/same unit cell is 3 times larger than the long/short axis radius. As a result, the CDM [1,56] is used to describe the interaction between the nanorods:
The optical response of each nanorod can be described by the polarizability using either an analytical [57] or semi-analytical [58] method. Here we directly use the multipole decomposition method [59–61] to give a precise description. This method is promising for describing nanoparticles with arbitrary shape and size. The dipole polarizability can be obtained as , where is the electric field along the long axis of the nanorod and is the total electric dipole moment calculated by the FDTD method (see subsection 2.B on FDTD simulation). The multipole decomposition analysis indicates that the total response of each nanorod is dominated by the total electric dipole moment, and higher multipoles are negligible.
Because of the periodicity in the plane of the metasurface, the Bloch theorem guarantees the solution of Eq. (1) must have the form and the incident electric field , including a phase factor involving the incident light’s momentum component parallel to a 2D metasurface. Specifically, is zero for normal incident light, i.e., , where is the electric field amplitude vector. We consider two cases of for left-/right-circularly polarized (LCP/RCP) light with electric amplitude vector . After some calculation, we have
If the wavelength is larger than the lattice constant (), then all terms of the sums are evanescent, except that for the , representing the electromagnetic wave propagating in the direction. If , the transmission has higher-order grating modes, whose directions are the same as . Finally, the far field of the (0,0) order grating mode [ and ] is
After solving the electric field, we can calculate the (0,0) order transmittance as
Note that the extinction cross section () in each unit cell is of the form
Similarly, the reflectance can be calculated as
The absorption of the metasurface is defined as . Then the absorption g-factor , and is the absorption in the presence of LCP/RCP. The analytical approach based on the CDM gives a clear physical picture, and the quantitative results are supported by the FDTD simulation as seen below.
B. FDTD Simulation
In FDTD simulation, the circularly polarized light is generated by the - and -direction polarized plane waves with phase difference. For a nanorod dimer, perfectly match layer (PML) boundary conditions are used in all boundaries of three dimensions. For metasurfaces, the PML boundary conditions are used in the direction, while periodic conditions are used in the and directions. The mesh cell is cube with size of 4 nm, and silver’s refractive index in the visible light range is obtained from Ref. [62].
To calculate the polarizability () of one single rod used in CDM, we use the multipole decomposition method [59–61] based on FDTD simulation of one rod:
3. RESULTS AND DISCUSSIONS
A. Optical Responses of a Single Nanorod Dimer and a Monolayer Metasurface: Localized Surface Plasmon Resonance and Lattice Resonance
Figure 2.Extinction cross sections of a dimer with twist angle
For comparison with new features of chiral optics due to LR in bilayer metasurfaces, we discuss the optical response of a monolayer metasurface made of silver nanorods with a rotational angle with respect to the axis. The CDM gives
In the presence of normally incident LCP/RCP light, the effective dipole moment is
Figure 3.Transmittances of monolayer metasurfaces with
B. Chiral Optical Response of Bilayer Metasurface: The Combination Effects from Lattice Resonance, PB Phase, and Propagation Phase
1. Chirality-Selective Transparency
As for bilayer metasurfaces, nanorods on the two layers may have different rotation angles and . So metasurface’s intrinsic chirality leads to different transmission for LCP and RCP light. The transmittances of a typical bilayer metasurface are displayed in Figs. 4(a) and 4(c) for those from FDTD simulation and CDM calculation. Different responses to LCP and RCP light are clearly seen, and there is very good agreement between the results from FDTD simulation and those based on CDM. Interestingly, a quite different response can be found as shown in Figs. 4(b) and 4(d) (for FDTD and CDM). Here one sees chirality-selective transparency. To understand the physics involved, it is helpful to rewrite Eq. (3) in the basis suitable for circularly polarized light. Then one has
In this case, . . Under the additional condition of , . Then identical transmittances for LCP and RCP light for all are obtained, which has been verified by FDTD simulation (not shown here).
Figure 4.Transmittance of a bilayer metasurface with parameters
We then discuss LR and the related Wood’s anomaly. From Eqs. (3) and (19), one can see that the quadratic terms of or in the denominator of () are zero. So the denominator and numerator only have linear terms of and . If , only is divergent. In general, the divergent terms in the denominator and numerator cancel each other out (“”), leading to the disappearance of Wood’s anomaly as seen in Figs. 4(a) and 4(c). Compared with the results of monolayer as shown in Fig. 3, the interlayer coupling generally destroys the Wood’s anomaly and related transparency, while in some specific conditions, the divergent terms in the numerator may be cancelled by the phase modulation. The coefficient in numerator for and is
Under the condition , the above coefficient for LCP or RCP (not both) vanishes, which leads to the recovery of the transparency induced by Wood’s anomaly for one of the circularly polarized lights. It is the chirality-selective transparency as seen in Fig. 4 (for , , and satisfying the condition). This transparency is obtained by modulating the PB phase and propagation phase [see Eq. (19)]. The nice agreement between the results from FDTD and CDM further verifies the analysis based on CDM.
From Eq. (21), one sees that the condition for chirality-selective transparency depends on the geometric parameters such as the twist angle and the separation between the nanorods. The phase-modulated lattice resonance and related chirality-selective transparency are the general effect. Changing the dimer length or the refractive index of the surrounding medium leads to a shift of the frequency of the LSPR of a single ellipsoid. The main physics of chirality-selective transparency remains unchanged.
Figure 5.(a), (b) Transmittance of a metasurface with achiral building blocks [i.e., unit cell with nanorod dimer of twist angle
In general, the phase states of transmission/reflection field depend on the detailed geometric parameters and wavelength, and the transmission and reflection waves are elliptically polarized. Using Eqs. (3), (10), and (12), one can see that at the lattice resonance (), transmission and reflection waves are circularly polarized with equal electric field amplitude in the direction for transmitted and reflected far fields. For the RCP incident field, transparency appears, and the transmitted wave possesses phase difference (phase of the electric field in the direction minus that in the direction) . For the LCP incident field, the transmission and reflection waves possess phase difference and .
2. Higher-Order Lattice Resonance
Figure 6.Transmittance of LCP/RCP light associated with higher-order resonance based on FDTD simulation. (a)
The conditions for the chirality-selective transparency related to higher-order lattice resonance () are
Here we would like to point out that the chirality-selective transparency associated with () is absent. Unlike the cases of LR under the conditions , both and are divergent for (). The coefficient of the term (, ) in the denominator is
3. Bilayer Metasurface with Square Lattice
The metasurface with a square lattice () possesses higher lattice symmetry than that with a rectangular lattice, which brings about new/different features in optical response. For the metasurface with a square lattice, and , and the effective dipole moments are
There is no chirality-selective transparency because the necessary condition of transparency eliminates the chirality of the structure.
In the following, we consider the case of . The term vanishes, indicating the effective decoupling of the upper and lower metasurfaces. Therefore, the bilayer metasurface shows achiral optical response like that of the monolayer metasurface. Also, the transparency due to Wood’s anomaly appears for both LCP and RCP light. From Eq. (24), we find that the scattering far field , with independent of or . In general, for the metasurface with a rectangular lattice in the presence of normally incident LCP/RCP field, the transmitted field contains both LCP and RCP components [see Eq. (19)]. For the metasurface with a square lattice in the presence of normally incident LCP/RCP field, the transmitted field contains only an LCP/RCP component. Moreover, the transmittance is independent of or .
4. Beyond Coupled Dipole Approximation
Figure 7.Transmittance of LCP/RCP light with
4. CONCLUSION
We theoretically explore the chiral optics of bilayer metasurfaces made of twisted nanorods, focusing on the collective effect due to LR. Through detailed analytical calculation based on CDM and FDTD simulations, we find that combination effects from LR and phase modulation (PB phase, propagation phase) can bring about novel chiral optical responses, including chirality-selective transparency (recovery of Wood’s anomaly) and chiral response for metasurfaces with achiral unit cells. The theoretical results deepen our understanding of light–matter interaction at the nanometer scale. In particular, the analytical results (supported by numerical simulation) give a quantitative relationship between local geometric structure, lattice structure, and their (chiral) optical properties; for example, the condition for chirality-selective transparency . Those special properties of metasurfaces could play important roles in optical communication, circular dichroism spectroscopy, and quantum information processing.
References
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